Efficient one-pot synthesis of alkyl levulinate from xylose with an integrated dehydration/transfer-hydrogenation/alcoholysis process,Sustainable Energy & Fuels

当前位置： X-MOL 学术 › Sustain. Energy Fuels › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Efficient one-pot synthesis of alkyl levulinate from xylose with an integrated dehydration/transfer-hydrogenation/alcoholysis process
Sustainable Energy & Fuels ( IF 5.0 ) Pub Date : 2019/12/18 , DOI: 10.1039/c9se00982e
Mengmeng Wang _{1,

2,

3,

4,

5} , Lincai Peng _{1,

2,

3,

4,

5} , Xueying Gao _{1,

2,

3,

4,

5} , Liang He _{1,

2,

3,

4,

5} , Junhua Zhang _{1,

2,

3,

4,

5}

Affiliation

An integrated catalytic protocol involving dehydration, transfer-hydrogenation and alcoholysis towards one-pot conversion of xylose to alkyl levulinate was invented using a combination of Zr(20)-MCM-41 and H₃O₄₀PW₁₂ catalysts. Secondary alcohols like 2-propanol and 2-butanol as the reaction medium exhibit equally superior hydrogen donating capability, but the dehydration step of xylose in 2-butanol is preferred probably due to its stronger hydrophobicity. A good alkyl levulinate yield of 53% can be achieved under optimized conditions. The spent dual catalysts can be effectively recovered and they exhibit good reusability after thermal regeneration of Zr(20)-MCM-41. Research on the catalytic mechanism shows that well-dispersed ZrO₂ supported on MCM-41 is responsible for the catalytic transfer hydrogenation step of furfural to furfuryl alcohol. Proper tuning of the Lewis and Brønsted acidities can efficiently promote the acid-driven reaction steps of xylose conversion and simultaneously inhibit the alkyl levulinate-to-γ-valerolactone side reaction. The sustainability of this conversion is greatly improved by process intensification based on the new catalytic strategy and mild reaction conditions.

中文翻译：

从木糖到脱水，转移，氢化，醇解一体化的高效一锅法合成乙酰丙酸烷基酯

结合Zr（20）-MCM-41和H ₃ O ₄₀ PW ₁₂催化剂，发明了一种涉及脱水，转移加氢和醇解向木糖到乙酰丙酸烷基酯一锅转化的综合催化方案。诸如2-丙醇和2-丁醇之类的仲醇作为反应介质表现出同样优异的给氢能力，但由于其较强的疏水性，因此优选木糖在2-丁醇中的脱水步骤。在最佳条件下，乙酰丙酸烷基酯的收率可达53％。Zr（20）-MCM-41的热再生后，可以有效地回收用过的双重催化剂，并且它们具有良好的可重复使用性。催化机理的研究表明，ZrO ₂分散均匀负载在MCM-41上的溶剂负责糠醛到糠醇的催化转移加氢步骤。适当调节Lewis和Brønsted的酸度可以有效地促进木糖转化的酸驱动反应步骤，同时抑制乙酰丙酸烷基酯到γ-戊内酯的副反应。通过基于新的催化策略和温和的反应条件的工艺强化，可以大大提高这种转化的可持续性。

更新日期：2020-03-03

点击分享查看原文

点击收藏

阅读更多本刊新发论文